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Photocatalytic uphill conversion of natural gas beyond the limitation of thermal reaction systems
Nature Catalysis ( IF 37.8 ) Pub Date : 2020-01-27 , DOI: 10.1038/s41929-019-0419-z
Shusaku Shoji , Xiaobo Peng , Akira Yamaguchi , Ryo Watanabe , Choji Fukuhara , Yohei Cho , Tomokazu Yamamoto , Syo Matsumura , Min-Wen Yu , Satoshi Ishii , Takeshi Fujita , Hideki Abe , Masahiro Miyauchi

Dry reforming of methane is one of the key reactions to exploit natural gas feedstocks by their catalytic conversion to synthesis gas (CH4 + CO2 → 2H2 + 2CO), which is used in the production of transportable liquid fuel. However, this reaction suffers from thermodynamic conversion limits and high thermal energy requirements. Herein we report that a SrTiO3-supported rhodium (Rh/STO) catalyst efficiently promotes methane reforming under ultraviolet light irradiation without heat supply at low temperatures, which cannot be achieved by conventional thermal catalysis. The photoexcited holes and electrons are used for CH4 oxidation over STO and CO2 reduction over rhodium, respectively. Isotope analysis clarified that the lattice oxygens (O2−) act as mediator to drive dry reforming of methane. The materials design of Rh/STO can be extended in principle to diverse uphill reactions that utilize photon energy to obtain valued products from different carbon resources.



中文翻译:

天然气的光催化上坡转化率超出了热反应系统的限制

甲烷的干重整是通过将天然气催化转化为合成气(CH 4  + CO 2  →2H 2  + 2CO)来开采天然气原料的关键反应之一,该天然气用于生产可运输的液体燃料。然而,该反应遭受热力学转化极限和高热能需求。在本文中,我们报道了SrTiO 3负载的铑(Rh / STO)催化剂有效地促进了在紫外线辐射下甲烷的重整,而没有低温供热,这是常规热催化无法实现的。光激发的空穴和电子用于CH 4在STO和CO 2上的氧化还原铑。同位素分析表明,晶格氧(O 2−)可作为媒介驱动甲烷的干重整。Rh / STO的材料设计原则上可以扩展到利用光子能量从不同碳资源中获得有价值产品的各种上坡反应。

更新日期:2020-01-27
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